In this article, polycrystalline samples of Gd3+ ion‐modified lead lanthanum zirconate titanate PLGZT: (Pb0.94‐xGdxLa0.06)(Zr0.52Ti0.48)O3; x = 0, 2, 4, 6, and 8% have been prepared by the sol‐gel autocombustion strategy. The structural properties of the prepared samples were analyzed by X‐ray diffraction profile (XRD), Fourier transform infrared spectra (FT‐IR), transmission electron microscopy (TEM), and scanning electron microscopy (SEM). The samples were assigned to pure PZT perovskite tetragonal structure. Ag electrodes were made on both sides of the disks for measurements of electrical and dielectric properties at different temperatures ranging from 30 to 500°C at various frequencies. The maximum dielectric constant, Curie temperature (TC), dielectric loss at TC, and the piezoelectric charge coefficient d33 ranges of the investigated samples were found to be 1850 to 2420, 350 to 399°C, 0.023 to 0.026, and 299 to 532 pC/N, respectively. Higher coefficients were reached for the 4 % Gd substitution. Finally, the obtained results indicate that these materials can be good candidates for ultrasonic transducers.